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Title: Hierarchically Structured MoO2/Dopamine-Derived Carbon Spheres as Intercalation Electrodes for Lithium-Ion Batteries

Journal Article · · Materials Today Chemistry
 [1];  [1];  [2];  [3];  [3];  [3];  [2];  [3];  [3];  [1]
  1. Drexel University, Philadelphia, PA (United States)
  2. Stony Brook University, NY (United States)
  3. Stony Brook University, NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

A hydrogen peroxide initiated sol-gel process involving molybdenum transformation in the presence of dopamine (Dopa) hydrochloride excess produced the metastable precipitate composed of polydopamine (PDopa) spheres coated with Dopa preintercalated molybdenum oxide, (Dopa)xMoOy@PDopa. The hydrothermal treatment (HT) of the (Dopa)xMoOy@PDopa precursor resulted in the simultaneous carbonization of Dopa and molybdenum reduction generating MoO2 nanoplatelets distributed and confined on the surface of the Dopa-derived carbon matrix (HT-MoO2/C). The consecutive annealing (An) of the HT-MoO2/C sample at 600 °C under Ar atmosphere led to the formation of MoO2 with increased Mo oxidation state and improved structural stability (AnHT-MoO2/C). Annealing had also further facilitated interaction between the molybdenum-derived and Dopa-derived components resulting in the modification of the carbon matrix confirmed by Raman spectroscopy. Morphology of both materials is best described as Dopa-derived carbon spheres decorated with MoO2 nanoplatelets. These integrated metal oxide and carbon structures were tested as electrodes for lithium-ion batteries in the potential window that corresponds to the intercalation mechanism of charge storage. The AnHT-MoO2/C electrode showed enhanced electrochemical activity, with an initial specific discharge capacity of 260 mAh/g and capacity retention of 67% after 50 cycles, compared to the HT-MoO2/C electrode which exhibited an initial specific discharge capacity of 235 mAh g–1 and capacity retention of 47% after 50 cycles. The rate capability experiments revealed that the capacity of 93 mAh/g and 120 mAh/g was delivered by the HT-MoO2/C and AnHT-MoO2/C electrodes, respectively, when the current density was increased to 100 mA/g. Here, the improved specific capacity, electrochemical stability, and rate capability achieved after annealing were attributed to higher crystallinity of MoO2, increased oxidation state of Mo, and formation of the tighter MoO2/carbon contact accompanied by the annealing assisted interaction between MoO2 and Dopa-derived carbon.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States); Northwestern Univ., Evanston, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
SC0012704; SC0012673; AC02-98CH10886; DMR-1752623; SC0021314
OSTI ID:
1896871
Alternate ID(s):
OSTI ID: 1865647
Report Number(s):
BNL-223649-2022-JAAM
Journal Information:
Materials Today Chemistry, Vol. 24; ISSN 2468-5194
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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